Tracing ancient solar cycles with tree rings and radiocarbon in the first millennium BCE.

The Sun drives Earth's energy systems, influencing weather, ocean currents, and agricultural productivity. Understanding solar variability is critical, but direct observations are limited to 400 years of sunspot records. To extend this timeline, cosmic ray-produced radionuclides like C in tree-rings provide invaluable insights.

Simultaneous Determination of Transuranium Radionuclides for Nuclear Forensics by Compact Accelerator Mass Spectrometry.

Accelerator mass spectrometry (AMS) is one of the most sensitive techniques used to measure the long-lived actinides. This is particularly of interest for determination of ultra-trace transuranium nuclides and their isotopic fingerprints for nuclear forensics. In this work, a new method was developed for simultaneous determination of transuranium nuclides (Np, Pu, Am, and Cm isotopes) by using 300 kV AMS after a sequential chemical separation of each group of actinides.

Time-Integrated Bioavailability Proxy for Actinides in a Contaminated Estuary.

Actinides accumulate within aquatic biota in concentrations several orders of magnitude higher than in the seawater [the concentration factor (CF)], presenting an elevated radiological and biotoxicological risk to human consumers. CFs currently vary widely for the same radionuclide and species, which limits the accuracy of the modeled radiation dose to the public through seafood consumption. We propose that CFs will show less dispersion if calculated using a time-integrated measure of the labile (bioavailable) fraction instead of a specific spot sample of bulk water.

Bioavailable actinide fluxes to the Irish Sea from Sellafield-labelled sediments.

Nuclear discharges to the oceans have given rise to significant accumulations of radionuclides in sediments which can later remobilise back into the water column. A continuing supply of radionuclides to aquatic organisms and the human food chain can therefore exist, despite the absence of ongoing nuclear discharges. Radionuclide remobilisation from sediment is consequently a critical component of the modelled radiation dose to the public.

Passive Sampling Tool for Actinides in Spent Nuclear Fuel Pools.

Spent nuclear fuel must be carefully managed to prevent pollution of the environment with radionuclides. Within the framework of correct radioactive waste management, spent fuel rods are stored in cooling pools to allow short-lived fission products to decay. If fuel rods leak, they liberate radionuclides into the cooling water; therefore, it is essential to determine radionuclide concentrations in the pool water for monitoring purposes and to plan the decommissioning process.

Tree-rings reveal two strong solar proton events in 7176 and 5259 BCE.

The Sun sporadically produces eruptive events leading to intense fluxes of solar energetic particles (SEPs) that dramatically disrupt the near-Earth radiation environment. Such events have been directly studied for the last decades but little is known about the occurrence and magnitude of rare, extreme SEP events. Presently, a few events that produced measurable signals in cosmogenic radionuclides such as C, Be and Cl have been found.

Cosmogenic radionuclides reveal an extreme solar particle storm near a solar minimum 9125 years BP.

During solar storms, the Sun expels large amounts of energetic particles (SEP) that can react with the Earth's atmospheric constituents and produce cosmogenic radionuclides such as C, Be and Cl. Here we present Be and Cl data measured in ice cores from Greenland and Antarctica. The data consistently show one of the largest Be and Cl production peaks detected so far, most likely produced by an extreme SEP event that hit Earth 9125 years BP (before present, i.

U/U Analysis of Femtograms of U by MC-ICPMS.

A new analytical method has been developed to determine atomic U/U ratios in samples with only femtograms of U using a secondary electron multiplier (SEM) on a multicollector high-resolution inductively coupled plasma mass spectrometer (MC-ICPMS). The abundance sensitivity of the U tail at 236 atomic mass unit is reduced from 10 to 10 with the deployment of a retarding potential quadrupole lens. This method features the reduction of polyatomic interferences from hydride, nitride, lead, and plutonium and the evaluation of nonlinear SEM behavior.

Cosmogenic in situ C-Be reveals abrupt Late Holocene soil loss in the Andean Altiplano.

Soil sustainability is reflected in a long-term balance between soil production and erosion for a given climate and geology. Here we evaluate soil sustainability in the Andean Altiplano where accelerated erosion has been linked to wetter climate from 4.5 ka and the rise of Neolithic agropastoralism in the millennium that followed.

Local and global trace plutonium contributions in fast breeder legacy soils.

Trace-level plutonium in the environment often comprises local and global contributions, and is usually anthropogenic in origin. Here, we report estimates of local and global contributions to trace-level plutonium in soil from a former, fast-breeder reactor site. The measured Pu/Pu ratio is anomalously low, as per the reduced Pu yield expected in plutonium bred with fast neutrons.

Lagged atmospheric circulation response in the Black Sea region to Greenland Interstadial 10.

Northern Hemispheric high-latitude climate variations during the last glacial are expected to propagate globally in a complex way. Investigating the evolution of these variations requires a precise synchronization of the considered environmental archives. Aligning the globally common production rate variations of the cosmogenic radionuclide Be in different archives provides a tool for such synchronizations.

U, Np and Pu as complementary fingerprints of radioactiveeffluents in the western Mediterranean Sea and in the Canada Basin (Arctic Ocean).

The aim of this study was to assess the potential of combining the conservatively behaving anthropogenic radionuclides U and Np to gain information on the origin of water masses tagged with liquid effluents from Nuclear Reprocessing Plants. This work includes samples collected from three full-depth water columns in two areas: i) the Arctic Ocean, where Atlantic waters carry the signal of Sellafield (United Kingdom) and La Hague (France) nuclear reprocessing facilities; and ii) the western Mediterranean Sea, directly impacted by Marcoule reprocessing plant (France). This work is complemented by the study of the particle-reactive Pu isotopes as an additional fingerprint of the source region.

Impact of nuclear fuel reprocessing on the temporal evolution of marine radiocarbon.

Radiocarbon (C) is broadly used in oceanography to determine water ages, trace water circulation, and develop sediment- and sclerochronologies. These applications require an accurate knowledge of marine C levels, which have been largely perturbed by human activities. Globally during the last century the above-ground nuclear weapon testings have been the primary cause of the increased atmospheric and marine C.

Unravelling 5 decades of anthropogenic U discharge from nuclear reprocessing plants.

Marine biogenic materials such as corals, shells, or seaweed have long been recognized as recorders of environmental conditions. Here, the bivalve Cerastoderma edule is used for the first time as a recorder of past seawater contamination with anthropogenic uranium, specifically U. Several studies have employed the authorized radioactive releases, including U, from nuclear reprocessing plants in La Hague, France, into the English Channel, and Sellafield, England, into the Irish Sea, to trace Atlantic waters and to understand recent climate induced circulation changes in the Arctic Ocean.

Multiradionuclide evidence for an extreme solar proton event around 2,610 B.P. (∼660 BC).

Recently, it has been confirmed that extreme solar proton events can lead to significantly increased atmospheric production rates of cosmogenic radionuclides. Evidence of such events is recorded in annually resolved natural archives, such as tree rings [carbon-14 (C)] and ice cores [beryllium-10 (Be), chlorine-36 (Cl)]. Here, we show evidence for an extreme solar event around 2,610 years B.

Tree rings reveal globally coherent signature of cosmogenic radiocarbon events in 774 and 993 CE.

Though tree-ring chronologies are annually resolved, their dating has never been independently validated at the global scale. Moreover, it is unknown if atmospheric radiocarbon enrichment events of cosmogenic origin leave spatiotemporally consistent fingerprints. Here we measure the C content in 484 individual tree rings formed in the periods 770-780 and 990-1000 CE.

Be-inferred paleo-denudation rates imply that the mid-Miocene western central Andes eroded as slowly as today.

Terrestrial cosmogenic nuclide concentrations of detrital minerals yield catchment-wide rates at which hillslopes erode. These estimates are commonly used to infer millennial scale denudation patterns and to identify the main controls on mass-balance and landscape evolution at orogenic scale. The same approach can be applied to minerals preserved in stratigraphic records of rivers, although extracting reliable paleo-denudation rates from Ma-old archives can be limited by the target nuclide's half-life and by exposure to cosmic radiations after deposition.

Anthropogenic U in the North Sea - A Closer Look into a Source Region.

In this study we present new seawater data of U and U sampled in the North Sea in 2010. The North Sea has been and is still receiving a considerable input of anthropogenic radionuclides from nuclear reprocessing facilities located in La Hague (France) and Sellafield (Great Britain). It therefore represents an important source region for oceanographic tracer studies using the transient signal of anthropogenic U.

Scavenged Pu, Pu, and Am from snowfalls in the atmosphere settling on Mt. Zugspitze in 2014, 2015 and 2016.

Concentrations of Pu, Pu, and Am, and atomic ratio of Pu/Pu in freshly fallen snow on Mt. Zugspitze collected in 2014, 2015 and 2016 were determined by accelerator mass spectrometry (AMS). For the sub-femtogram (10 g) - level of Pu and Am analysis, a chemical separation procedure combined with AMS was improved and an excellent overall efficiency of about 10 was achieved.

Potential Releases of I, U, and Pu Isotopes from the Fukushima Dai-ichi Nuclear Power Plants to the Ocean from 2013 to 2015.

After the Fukushima Dai-ichi nuclear accident, many efforts were put into the determination of the presence of Cs, Cs, I, and other gamma-emitting radionuclides in the ocean, but minor work was done regarding the monitoring of less volatile radionuclides, pure beta-ray emitters or simply radionuclides with very long half-lives. In this study we document the temporal evolution of I, U, and Pu isotopes (Pu and Pu) in seawater sampled during four different cruises performed 2, 3, and 4 years after the accident, and we compare the results to Cs collected at the same stations and depths. Our results show that concentrations of I are systematically above the nuclear weapon test levels at stations located close to the FDNPP, with a maximum value of 790 × 10 at·kg, that exceeds all previously reported I concentrations in the Pacific Ocean.

Laser Ablation - Accelerator Mass Spectrometry: An Approach for Rapid Radiocarbon Analyses of Carbonate Archives at High Spatial Resolution.

A new instrumental setup, combining laser ablation (LA) with accelerator mass spectrometry (AMS), has been investigated for the online radiocarbon ((14)C) analysis of carbonate records. Samples were placed in an in-house designed LA-cell, and CO2 gas was produced by ablation using a 193 nm ArF excimer laser. The (14)C/(12)C abundance ratio of the gas was then analyzed by gas ion source AMS.

Probing the Kinetic Parameters of Plutonium-Naturally Occurring Organic Matter Interactions in Freshwaters Using the Diffusive Gradients in Thin Films Technique.

The interaction of trace metals with naturally occurring organic matter (NOM) is a key process of the speciation of trace elements in aquatic environments. The rate of dissociation of metal-NOM complexes will impact the amount of free metal available for biouptake. Assessing the bioavailability of plutonium (Pu) helps to predict its toxic effects on aquatic biota.

Determination of Atto- to Femtogram Levels of Americium and Curium Isotopes in Large-Volume Urine Samples by Compact Accelerator Mass Spectrometry.

Ultralow level analysis of actinides in urine samples may be required for dose assessment in the event of internal exposures to these radionuclides at nuclear facilities and nuclear power plants. A new bioassay method for analysis of sub-femtogram levels of Am and Cm in large-volume urine samples was developed. Americium and curium were co-precipitated with hydrous titanium oxide from the urine matrix and purified by column chromatography separation.

Speciation and Bioavailability Measurements of Environmental Plutonium Using Diffusion in Thin Films.

The biological uptake of plutonium (Pu) in aquatic ecosystems is of particular concern since it is an alpha-particle emitter with long half-life which can potentially contribute to the exposure of biota and humans. The diffusive gradients in thin films technique is introduced here for in-situ measurements of Pu bioavailability and speciation. A diffusion cell constructed for laboratory experiments with Pu and the newly developed protocol make it possible to simulate the environmental behavior of Pu in model solutions of various chemical compositions.